Land surface albedo, qualifying the ratio of the radiant flux reflected from the land surface to the incident flux, is a key forcing parameter controlling the Earth’s energy budget. Previously, several BRDF archetypes were distilled from high-quality MODIS BRDF/Albedo products. In this study, we propose a method that largely relies on matching observed multiangular reflectances with the most appropriate of these prior BRDF archetypes to determine the amplitude and shape of the actual surface BRDFs, when directional signatures are insufficient. This method is first evaluated using an assortment of multisource BRDF data sets to demonstrate its viability for surface albedo estimates, and then is applied to airborne wide-angle infrared dual-mode line/area array scanner (WIDAS) from the Watershed Allied Telemetry Experimental Research (WATER) campaign in the Heihe River Basin of China in 2008. This algorithm makes use of the linear MODIS BRDF model to determine the BRDF archetypes needed as prior knowledge for intrinsic spectral albedo estimates. The intrinsic spectral albedos are then used to estimate actual spectral albedos by considering the proportion of direct and diffuse solar radiation. A spectral-to-broadband conversion is performed to generate the broadband albedo at shortwave regimes through the use of conversion coefficients derived from extensive radiative transfer simulations. A further validation confirms that the estimated albedos are consistent with in situ field measured albedos over available corn crop sites. This method provides a major advantage on utilizing generalized BRDF information derived from MODIS in conjunction with other instrument data that are acquired with less angular variation.